磷空位工程化的Ru,Pv-CoP作为氢溢流催化剂以增强工业碱性水电解

doi:10.1016/S1872-2067(26)65195-9

催化学报 ›› 2026, Vol. 91: 192-209.DOI: 10.1016/S1872-2067(26)65195-9

磷空位工程化的Ru,P_v-CoP作为氢溢流催化剂以增强工业碱性水电解

肖娟^a, 黄婷婷^a, 刘夏^a, 冯玉莹^a, 许贯诚^a^,^*(), 张丽^b^,^*()

^a 新疆大学化学学院, 碳基能源化学与利用国家重点实验室, 新疆乌鲁木齐 830017
^b 新疆大学化工学院, 新疆乌鲁木齐 830017

收稿日期:2026-01-07 接受日期:2026-04-16 出版日期:2026-12-18 发布日期:2026-10-13
通讯作者: ^*电子信箱: xuguancheng@xju.edu.cn (许贯诚),
zhangli420@xju.edu.cn (张丽).
基金资助:
新疆人才发展基金(XJRC-2025-KJ-PY-KJLJ-042);新疆维吾尔自治区研究生科研创新项目(XJ2025G022)

Phosphorus vacancy-engineered Ru,P_v-CoP as a hydrogen spillover catalyst for enhanced industrial alkaline water electrolysis

Juan Xiao^a, Tingting Huang^a, Xia Liu^a, Yuying Feng^a, Guancheng Xu^a^,^*(), Li Zhang^b^,^*()

^a State Key Laboratory of Chemistry and Utilization of Carbon-Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, Xinjiang, China
^b College of Chemical Engineering, Xinjiang University, Urumqi 830017, Xinjiang, China

Received:2026-01-07 Accepted:2026-04-16 Online:2026-12-18 Published:2026-10-13
About author:First author contact:CRediT authorship contribution statement
Juan Xiao: Conceptualization, Methodology, Formal analysis, Writing-original draft, Writing-review & editing. Tingting Huang: Writing-review & editing. Xia Liu: Writing-review & editing. Yuying Feng: Writing-review & editing. Guancheng Xu: Funding acquisition, Writing-review & editing, Supervision. Li Zhang: Writing-review & editing.
Supported by:
Xinjiang Talent Development Fund(XJRC-2025-KJ-PY-KJLJ-042);Graduate Research Innovation Pro-ject of Xinjiang Uygur Autonomous Region(XJ2025G022)

摘要/Abstract

摘要：

在全球碳中和背景下, 碱性水电解(AWE)是绿氢供应的核心技术. 然而, 阴极析氢反应(HER)的缓慢动力学是制约其效率提升的核心瓶颈. 经典HER作用机制普遍受限于“标度关系”, 单一活性位点难以同步优化水吸附/解离、氢吸附、氢气脱附等多步基元反应, 进而导致HER反应速率不佳. 氢溢流(HSo)效应为破解该难题提供了全新思路, 通过不同活性位点间的接力催化, 可显著提升碱性条件下的HER动力学. 现阶段, HSo的调控方式多聚焦于异质结构筑、功函数调控、缩短传质路径及单原子催化剂设计等常规手段, 而通过精准缺陷工程定向调控HSo效应、赋能高效HER催化的研究仍较为匮乏, 相关机理探究与体系开发缺乏系统性、深层次剖析.
本文借助缺陷工程策略, 采用水热-刻蚀-浸渍-低温磷化四步法在CoP表面锚定Ru纳米晶(NCs)和Ru单原子(SAs), 成功制备出具有丰富磷空位的新型氢溢流催化材料(Ru,P_v-CoP). 系统探究并阐明了磷空位在调控HSo效应, 进而提升HER催化活性的关键作用与内在机理. 结合X-射线光电子能谱、同步辐射等结果表明, 磷空位可有效调控Ru活性物种与CoP基底的界面理化性质, 通过Ru-P-Co桥联键合作用实现Ru、Co双位点间的强电子耦合, 成功构筑了“Ru-Co”“供体-受体”电子对. 依托其独特的电子构型, 多维原位电化学表征测试结果证实, 磷空位可显著加速水分子的富集与极化解离, 同时促进吸附态中间体(H*)的捕获与迁移. 密度泛函理论计算进一步揭示, 磷空位极大缩小了Ru NCs与Ru_SA-CoP之间的功函数差, 强化Ru NCs向Co位点的电子供给, 进而实现H*的高效跨相传输. 在催化反应中, Ru NCs主要驱动水分子解离, 所生成的H*通过HSo效应迁移至邻近Co位点, 经历重组完成氢气脱附. 得益于磷空位介导的双位点接力催化机制, Ru,P_v-CoP/CF在1.0 mol L^-1 KOH溶液中展现出优异的HER催化性能. 工业级大电流密度(1.0 A cm^-2)下, HER过电位仅为86 mV. 同时, 该催化剂兼具优异的析氧(OER)反应活性, 相同工业电流密度条件下的OER过电位低至350 mV. 凭借其HER/OER双功能催化协同优势, 该催化剂在阴离子交换膜电解水装置中表现出优异的催化活性与长周期稳定性. 60 °C, 1.0 A cm^-2电流密度的工况下, 电解槽电压仅为1.89 V, 可稳定运行长达275 h, 综合性能优于大多数已报道的自支撑过渡金属磷化物催化剂, 具备良好的工业化应用前景. 此外, 磷空位的引入可显著优化活性位点分布, 大幅提高贵金属Ru的原子利用效率, 实现贵金属质量活性的成倍提升.
综上, 本研究通过精准可控的空位工程策略, 在过渡金属磷化物催化体系中成功构筑了高效、定向的氢溢流传输通道. 本文不仅深化了空位调控氢溢流机制的理论认知, 更为破解工业碱性水电解体系中多步反应动力学耦合受限的核心难题, 提供了全新的材料设计思路与理论参考范式.

关键词: 氢溢流, 磷空位, 钌纳米晶, 过渡金属磷化物, 工业碱性水电解

Abstract:

Developing industrial-grade electrocatalysts based on the hydrogen spillover (HSo) mechanism is a key approach for translating lab-scale performance into industrial applications. Herein, a novel HSo catalyst (Ru,P_v-CoP/CF) was constructed by introducing phosphorus vacancies (P_v) into a CoP support decorated with Ru nanocrystals (Ru NCs) and Ru single atoms (Ru SAs) via defect-engineering strategy. The creation of P_v modulates the interfacial properties between Ru species and CoP, enabling electronic coupling between Ru and Co through phosphorus bridging and forming a “Ru-Co” donor-acceptor electron pair. Multidimensional in-situ electrochemical measurements reveal that P_v accelerates the polarization/dissociation of water molecules and the capture/migration of adsorbed hydrogen (H*). Further density functional theory calculations underscore that P_v narrows the work function difference between Ru NC and Ru_SA-CoP, which enhances the electron supply from Ru NC to Co, thereby triggering an efficient H* cross-phase transmission. Specifically, Ru NCs primarily facilitate H₂O dissociation, and the generated H* subsequently spillover to adjacent Co sites for H₂ desorption. Benefiting from the P_v-mediated relay catalysis, the Ru,P_v-CoP/CF catalyst exhibits top-level HER properties in 1.0 mol L^-1 KOH, requiring only 86 mV at an industrial current density of 1.0 A cm^-2 with exceptional durability over 1200 h. This work advances the fundamental understanding of vacancy-guided HSo mechanism, providing unique insights for designing transition metal phosphides-based electrocatalysts for industrial alkaline water electrolysis.

Key words: Hydrogen spillover, Phosphorus vacancies, Ru nanocrystals, Transition metal phosphides, Industrial alkaline water electrolysis

肖娟, 黄婷婷, 刘夏, 冯玉莹, 许贯诚, 张丽. 磷空位工程化的Ru,P_v-CoP作为氢溢流催化剂以增强工业碱性水电解[J]. 催化学报, 2026, 91: 192-209.

Juan Xiao, Tingting Huang, Xia Liu, Yuying Feng, Guancheng Xu, Li Zhang. Phosphorus vacancy-engineered Ru,P_v-CoP as a hydrogen spillover catalyst for enhanced industrial alkaline water electrolysis[J]. Chinese Journal of Catalysis, 2026, 91: 192-209.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65195-9

https://www.cjcatal.com/CN/Y2026/V91/I12/192

图/表 8

Scheme 1. Schematic illustration of the synthesis of Ru,Pv-CoP/CF.

Fig. 1. XRD (a), SEM (b,c), TEM (d), AC-STEM (e-h), EELS (i), and TEM-elemental mapping (l-p) images of Ru,Pv-CoP/CF.

Fig. 2. High-resolution XPS spectra of Co 2p (a), P 2p (b) for Ru,Pv-CoP/CF and CoP/CF. (c) Ru 3p for Ru,Pv-CoP/CF and Ru-CoP/CF. EPR spectra (d), the normalized Co K-edge XANES spectra (e) and FT-EXAFS spectra (f) of Ru,Pv-CoP/CF, Ru-CoP/CF, CoP/CF, Co foil and Co2O3. WT-EXAFS spectra for Co K-edge (g), the normalized Ru K-edge (h) XANES spectra, the FT-EXAFS spectra (i-j) of Ru,Pv-CoP/CF, Ru-CoP/CF, Ru foil, RuCl3 and RuO2. WT-EXAFS spectra for Ru K-edge (k) and the R space comparison chart (l) for Ru,Pv-CoP/CF and Ru-CoP/CF. (m) Schematics of the electronic coupling in the Ru-Pv··-Co bridge.

Fig. 3. (a) iR-corrected LSV curves of HER. (b) Overpotentials at current density of 50, 100, 500 and 1000 mA cm-2. (c) Comparison of overpotentials (at 1 A cm-2) and Tafel slopes of various reported self-supported TMP-based HER catalysts. Tafel slope plots (d), double-layer capacitances (e), Nyquist plots (f), and TOF curves (g) of Ru,Pv-CoP/CF, Ru-CoP/CF, Pv-CoP/CF and CoP/CF. (h) TOF values comparison at an overpotential of 100 mV. (i) Mass activity of Ru,Pv-CoP/CF and Ru-CoP/CF. (j) Mass activity comparison at an overpotential of 100 mV. (k) Chronopotentiometric E-t test of Ru,Pv-CoP/CF.

Fig. 4. (a) HER LSV curves of Ru,Pv-CoP/CF in 1.0 mol L-1 KOH electrolyte with various pH. (b) The linear plots of log|j@-50 mV vs. RHE| versus pH for Ru,Pv-CoP/CF, Ru-CoP/CF, Pv-CoP/CF and CoP/CF. (c) CV curves of Ru,Pv-CoP/CF. (d) Plots of hydrogen desorption peak position versus scan rates of the Ru,Pv-CoP/CF and Ru-CoP/CF. (e) EIS-derived Tafel plots. (f) Plots of Cϕ versus η. (g,h) In-situ Raman of Ru,Pv-CoP/CF and Ru-CoP/CF catalysts in 1.0 mol L-1 KOH under various potentials (V vs. RHE). (i-k) Evolution of interfacial water configurations at the interface of Ru,Pv-CoP/CF and Ru-CoP/CF with applied potentials. (l) In-situ ATR-FTIR spectra of Ru,Pv-CoP/CF in 0.1 mol L-1 KOH solution.

Fig. 5. Calculated DOS plots of CoP (a), Ru,Pv-CoP (b). (c) PDOS of Co 3d orbitals of CoP and Ru,Pv-CoP. (d) The work function between the Ru NC, RuSA-CoP and RuSA,Pv-CoP. (e) Planar average potential along the Z-direction. (f) The charge-density difference at the interface. H2O adsorption energy (ΔEH2O*) (g), H2O dissociation (h) and H-adsorption (i) of each system. (j) Hydrogen adsorption transfer pathway diagram. (k) Schematic diagram of the enhanced HER mechanism for Ru,Pv-CoP.

Fig. 6. (a) iR-corrected LSV curves of OER. (b) Overpotentials at current density of 50, 100, 500 and 1000 mA cm-2. (c) Comparison of overpotentials (at 1 A cm-2) and Tafel slopes of various reported self-supported TMP-based OER catalysts. Tafel slope plots (d), double-layer capacitances (e), Nyquist plots (f), operando-EIS tests (g-l) of Ru,Pv-CoP/CF, Ru-CoP/CF, Pv-CoP/CF and CoP/CF. (m) Potential dependence of the phase angle. (n) Chronopotentiometric E-t test of Ru,Pv-CoP/CF.

Fig. 7. AEMWE device performance. (a) Schematic of the AEMWE device. (b) Polarization curves of Ru,Pv-CoP/CF‖Ru,Pv-CoP/CF paired electrodes for AEMWE under 25 °C and 60 °C. (c) The voltage comparison at different current densities. (d,e) Long-term stability of the AEMWE system at 1 A cm-2 under 25 and 60 °C. (f) The comparison of the AEMWE performance of this work with other electrocatalysts reported to date.

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磷空位工程化的Ru,P_v-CoP作为氢溢流催化剂以增强工业碱性水电解

Phosphorus vacancy-engineered Ru,P_v-CoP as a hydrogen spillover catalyst for enhanced industrial alkaline water electrolysis

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磷空位工程化的Ru,Pv-CoP作为氢溢流催化剂以增强工业碱性水电解

Phosphorus vacancy-engineered Ru,Pv-CoP as a hydrogen spillover catalyst for enhanced industrial alkaline water electrolysis

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磷空位工程化的Ru,P_v-CoP作为氢溢流催化剂以增强工业碱性水电解

Phosphorus vacancy-engineered Ru,P_v-CoP as a hydrogen spillover catalyst for enhanced industrial alkaline water electrolysis